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Despite the variety of available computational approaches, state-of-the-art methods for calculating excitation energies such as time-dependent density functional theory (TDDFT), are computationally demanding and thus limited to moderate…

Chemical Physics · Physics 2022-03-10 Martina Stella , Kritam Thapa , Luigi Genovese , Laura E. Ratcliff

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical…

Materials Science · Physics 2022-09-12 Marcus Annegarn , Juhan Matthias Kahk , Johannes Lischner

The self-consistent field theory (SCFT) is a powerful framework for the study of the phase behavior and structural properties of many-body systems. In particular, polymeric SCFT has been successfully applied to inhomogeneous polymeric…

Soft Condensed Matter · Physics 2019-01-31 An-Chang Shi

For the computational prediction of core electron binding energies in solids, two distinct kinds of modelling strategies have been pursued: the $\Delta$-Self-Consistent-Field method based on density functional theory (DFT), and the GW…

Materials Science · Physics 2023-06-12 Juhan Matthias Kahk , Johannes Lischner

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert

We present a detailed comparison of the S0, S1 (n -> \pi*) and S2 (\pi -> \pi*) potential energy surfaces (PESs) of the prototypical molecular switch azobenzene as obtained by Delta-self-consistent-field (Delta-SCF) Density-Functional…

Chemical Physics · Physics 2012-02-22 Reinhard J. Maurer , Karsten Reuter

Constrained-occupancy self-consistent-field ($\Delta$SCF) methods and many-body perturbation theories (MBPT) are two strategies for obtaining electronic excitations from first-principles. Using the two distinct approaches, we study the O…

Materials Science · Physics 2017-03-08 Yufeng Liang , John Vinson , Sri Pemmeraju , Walter Drisdell , Eric Shirley , David Prendergast

Self-consistent field theory (SCFT) is one of the useful methods to simulate phase separated structures of multi-component polymer systems. In this article, we propose an SCFT for semiflexible polymer melts, where the basic equations for…

Soft Condensed Matter · Physics 2025-03-04 Yutaka Oya , Toshihiro Kawakatsu

Delta self-consistent-field ($\Delta$SCF) theory is widely used for electronic excitation energy calculations. However, calculating the corresponding oscillator strengths is challenging. The corresponding many-electron wavefunctions are not…

Chemical Physics · Physics 2026-03-18 Yang Shen , Yichen Fan , Weitao Yang

In this work, we revisited the idea of using the coupled-cluster ground state formalism to target excited states. Our main focus was targeting doubly excited states and double core hole states. Typical equation-of-motion (EOM) approaches…

Chemical Physics · Physics 2019-12-04 Joonho Lee , David W. Small , Martin Head-Gordon

The Tamm-Dancoff Approximation (TDA) offers a computationally efficient alternative to full linear-response Time-Dependent Density Functional Theory (TDDFT) for calculating electronic excited states, particularly in large molecular systems.…

Chemical Physics · Physics 2025-07-02 Muhammed A. Dada , Sarah Pak , Matthew N. Ward , Megan Simons , Daniel R. Nascimento

The $\Delta$-Self-Consistent-Field ($\Delta$SCF) method permits calculations of core electron binding energies in materials and molecules at a modest computational cost. However, it has been reported that whilst this method works well for…

We present a formulation of spin-conserving and spin-flip, hybrid time-dependent density functional theory (TDDFT), including the calculation of analytical forces, which allows for efficient calculations of excited state properties of…

Materials Science · Physics 2023-12-05 Yu Jin , Victor Wen-zhe Yu , Marco Govoni , Andrew C Xu , Giulia Galli

The $\Delta$-Self-Consistent-Field ($\Delta$SCF) method has been established as an accurate and computationally efficient approach for calculating absolute core electron binding energies for light elements up to chlorine, but relatively…

Materials Science · Physics 2022-10-12 Juhan Matthias Kahk , Johannes Lischner

Charge-transfer excited states are highly relevant for applications in molecular electronics. However, the accurate calculation of these states in large systems is challenging since wave function methods are prohibitively expensive,…

Chemical Physics · Physics 2025-05-20 Nicola Bogo , Zeyi Zhang , Martin Head-Gordon , Christopher J. Stein

We present a mean field theory for excited states that is broadly analogous to ground state Hartree-Fock theory. Like Hartree-Fock, our approach is deterministic, state-specific, applies a variational principle to a minimally correlated…

Strongly Correlated Electrons · Physics 2018-08-28 Jacqueline A. R. Shea , Eric Neuscamman

Molecules that have been suggested to violate the Hund's rule, having a first excited singlet state (S$_1$) energetically below the triplet state (T$_1$), are rare. Yet, they hold the promise to be efficient light emitters. Their…

Chemical Physics · Physics 2025-09-23 Atreyee Majumdar , Raghunathan Ramakrishnan

Recent work from our research group has demonstrated that symmetry-projected Hartree--Fock (HF) methods provide a compact representation of molecular ground state wavefunctions based on a superposition of non-orthogonal Slater determinants.…

Chemical Physics · Physics 2015-06-17 Carlos A. Jiménez-Hoyos , R. Rodríguez-Guzmán , Gustavo E. Scuseria

Time-dependent density functional theory (TDDFT) is presently enjoying enormous popularity in quantum chemistry, as a useful tool for extracting electronic excited state energies. This article explains what TDDFT is, and how it differs from…

Materials Science · Physics 2007-05-23 Peter Elliott , Kieron Burke , Filipp Furche